Hydration structure and water exchange reaction of Nickel(II) ion: Classical and QM/MM Simulations

被引:58
作者
Inada, Y [1 ]
Mohammed, AM
Loeffler, HH
Rode, BM
机构
[1] Univ Innsbruck, Dept Theoret Chem, Inst Gen Inorgan & Theoret Chem, A-6020 Innsbruck, Austria
[2] Nagoya Univ, Res Ctr Mat Sci, Nagoya, Aichi 4648602, Japan
[3] Univ Addis Ababa, Dept Chem, Addis Ababa, Ethiopia
关键词
D O I
10.1021/jp0155314
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Classical molecular dynamics (MD), classical Monte Carlo (MC), and combined quantum mechanical/molecular mechanical (QM/MM) MD simulations were carried out to investigate the hydration structure of the Ni(II) ion in water using a newly constructed 2-body potential and a function correcting for 3-body effects. A 6-coordinate hydration structure with a maximum probability of the Ni-O distance at 2.25, 2.21, and 2.14 Angstrom was observed by the classical MD, classical MC, and QM/MM-MD simulation with 3-body corrections, respectively, while an 8-coordinate structure was observed by the classical MD and MC simulations using only 2-body pair potentials. The average structure parameters obtained by the Hertree-Fock level QM/MM-MD simulation are in agreement with the experimental values. The validity of the 3-body correction function is discussed on the basis of the results for the classical and QM/MM simulations. During the classical MD simulation, a water exchange reaction was observed for the 6-coordinate Ni(II) ion. The water exchange reaction proceeded via a 5-coordinate intermediate with the lifetime of ca. 2.5 ps. The observed dissociative mechanism of the water exchange reaction is in accordance with experimental evidence.
引用
收藏
页码:6783 / 6791
页数:9
相关论文
共 100 条
[81]   Molecular dynamics simulations of Ca2+ in water:: Comparison of a classical simulation including three-body corrections and Born-Oppenheimer ab initio and density functional theory quantum mechanical/molecular mechanics simulations [J].
Schwenk, CF ;
Loeffler, HH ;
Rode, BM .
JOURNAL OF CHEMICAL PHYSICS, 2001, 115 (23) :10808-10813
[82]   TRANSITION STRUCTURE AND SUBSTITUENT EFFECTS ON AQUEOUS ACCELERATION OF THE CLAISEN REARRANGEMENT [J].
SEHGAL, A ;
SHAO, L ;
GAO, JL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1995, 117 (45) :11337-11340
[83]   Three-body effects in calcium(II)-ammonia solutions: Molecular dynamics simulations [J].
Sidhisoradej, W ;
Hannongbua, S ;
Ruffolo, D .
ZEITSCHRIFT FUR NATURFORSCHUNG SECTION A-A JOURNAL OF PHYSICAL SCIENCES, 1998, 53 (05) :208-216
[84]   Pressure dependence and activation volume for the water exchange mechanism in NaCl(aq) from MD simulations [J].
Spangberg, D ;
Wojcik, M ;
Hermansson, K .
CHEMICAL PHYSICS LETTERS, 1997, 276 (1-2) :114-121
[85]   REVISED CENTRAL FORCE POTENTIALS FOR WATER [J].
STILLINGER, FH ;
RAHMAN, A .
JOURNAL OF CHEMICAL PHYSICS, 1978, 68 (02) :666-670
[86]   Coupled QM/MM molecular dynamics simulations of HCl interacting with ice surfaces and water clusters - Evidence of rapid ionization [J].
Svanberg, M ;
Pettersson, JBC ;
Bolton, K .
JOURNAL OF PHYSICAL CHEMISTRY A, 2000, 104 (24) :5787-5798
[87]   MONTE-CARLO SIMULATIONS OF CU(II) IN WATER WITH 3-BODY POTENTIAL [J].
TEXLER, NR ;
RODE, BM .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (43) :15714-15717
[88]   The hydration shell structure of Li+ investigated by Born-Oppenheimer ab initio QM/MM dynamics [J].
Tongraar, A ;
Liedl, KR ;
Rode, BM .
CHEMICAL PHYSICS LETTERS, 1998, 286 (1-2) :56-64
[89]   Born-Oppenheimer ab initio QM/MM dynamics simulations of Na+ and K+ in water:: From structure making to structure breaking effects [J].
Tongraar, A ;
Liedl, KR ;
Rode, BM .
JOURNAL OF PHYSICAL CHEMISTRY A, 1998, 102 (50) :10340-10347
[90]   Solvation of Ca2+ in water studied by Born-Oppenheimer ab initio QM/MM dynamics [J].
Tongraar, A ;
Liedl, KR ;
Rode, BM .
JOURNAL OF PHYSICAL CHEMISTRY A, 1997, 101 (35) :6299-6309